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A magnetic resonance (MR)-fluorescent dual-mode imaging probe was prepared by conjugating guaiazulene to Gd-DOTA, and used to label human mesenchymal stem cells (hMSCs) via electroporation. The probe self-assembled into nanoclusters in the cytoplasm, resulting in a significant reduction in T2-weighted signal intensity that persisted up to 7 days. The fluorescence signal of the probe was observed at 498 nm, and the labelled hMSCs emitted a green fluorescence. The MR-fluorescent dual-mode imaging probe can potentially be used for stem cell tracking in vivo.